摘要：A reasonable design strategy to improve the utilization of noble metal electrocatalysts for the hydrogen evolution reaction(HER)is crucial to simplify the process flow and accelerate the future renewable energy ***,abundant defects were created on 2.4-nm Ru nanoparticles to achieve unprecedently high mass-specific reactivity in harsh acidic and alkaline *** obtained defect-enriched Ru(DR-Ru)exhibits an ultrahigh HER turnover frequency of16.4 s^(-1)with a 100-mV overpotential in alkaline media,and it also retains an excellent value of 20.6 s^(-1)in acidic media;these results are superior to those reported for other Ru ***,a record-low loading of 2.5μg cm^(-2)for the DR-Ru catalysts and low overpotentials of 28.2 and 25.1 mV at10 mA cm^(-2)can be realized in alkaline and acidic media,***,the less coordinated Ru surface sites and partial lattice oxygen introduction weaken the bonding between H and DR-Ru catalysts,facilitate fast acidic HERkinetics and help dissociate the water molecule to overcome the major challenge of HER in alkaline electrolytes,leading to an activity comparable to that under acidic *** result provides a guideline for defect engineering on noble metal nanocatalysts to effectively improve the utilization of the catalysts and optimize reactivities.

摘要：电化学界面动力学决定了所有电化学反应性质.从原子和分子水平上多维度原位观察电极的表界面电化学反应动态过程对于典型的电化学储能技术(电解槽、燃料电池)中催化剂的结构设计、合成和筛选具有重要意义,但是复杂的电化学界面以及微量、快速的反应中间态信号给界面电化学反应动态过程研究带来了极大的挑战.同步辐射傅里叶变换红外光谱(SR-FTIR)具有独特的分子指纹识别功能,可以用来确定电化学界面的活性物质,结合对纳米材料的局部原子结构高度敏感的同步辐射X射线吸收精细结构(SR-XAFS)光谱可以开展界面电化学反应过程的实时动态研究,有助于指导设计用于高效高能量密度能源系统的先进电催化剂.本文基于近年来本课题组的研究工作,系统地介绍了获得高质量的电化学反应过程中同步辐射红外关联谱学实验结果的策略,及其应用于电催化反应动态过程研究成果,其中主要选用当前热门的金属有机框架(MOF)纳米材料以及金属单原子催化剂(SACs)作为研究对象.最后,对原位同步辐射实验方法发展及其针对电化学反应动态过程的研究进行了展望,旨在通过揭示电化学反应的动态机理来指导和合成高效稳定的催化材料.